上海市冬季大气中PBDEs的分布及趋势分析
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摘要
利用被动采样器采集了上海地区15个采样点冬季的大气样品,对其进行索氏提取和层析净化等前处理后采用GC-MS进行定性定量分析,10种待测多溴联苯醚(PBDEs)目标化合物均被检出。将2008、2013和2014三个年度上海市冬季大气PBDEs监测结果进行比较分析,各年度的∑_(10)PBDEs质量浓度均值分别为5.7 pg/m~3、17.28pg/m~3和61.31 pg/m~3,在监测年限内有明显的上升趋势。经同系物分析,低溴代物(五溴代物以下)为上海大气中的主要污染物,其中BDE-49与BDE-47贡献较大,占到了总质量浓度的45.39%和24.68%,是主要的污染同系物。对监测点分区比较发现,上海城区的∑_(10)PBDEs质量浓度明显高于郊区。
In order to investigate the actual spatial atmospheric distribution situation in-situ of the pollutants of the polybrominated diphenyl ethers(PBDEs) in Shanghai,we have chosen 15 sampling points in the city in winter.To achieve the goal of our investigation,we have first of all managed to collect the air samples,that is,the PUF(polyurethane foam) passive air samplers for the 3 months in the winter season(from December,2013,to March,2014).And,then,we have managed to make the collected samples treated with Soxhlet extraction and chromatographic purification(pretreated in the lab condition),both in qualitative and quantitative ways,to work out the following 10 targeted components,that is,those of PBDEs(BDE-17,PBEB,BDE-49,BDE-47,BDE-100,BDE-99,BDE-85,BDE-154,BDE- 153 and BDE- 138) respectively in a content concentration range of ∑_(10)PBDEs from 24.18 pg/m~3 to 83.26 pg/m~3,with the mean value of ∑_(10) PBDEs being 61.31 pg/m~3,whereas the average concentrations of ∑_7 PBDEs(BDE- 47,BDE- 99,BDE- 100,BDE-28,BDE- 153,BDE- 154 and BDE- 183) are8.44 pg/m~3(laboratory test of 7 kinds of homologues).The results of the comparative analysis of all the said samples aforementioned show that ∑_(10) PBDEs means in each year are 5.7 pg/m~3,17.28 pg/m~3 and 61.31 pg/m~3 respectively,which represents a clear growing trend during the aforementioned monitoring period.That is to say,the total amount of PBDEs remains in the growing trend for the short term,the long term variation of PBDEs levels will be continued in the near future in the said region.What is more,we have also made a brief analysis of the sources of PBDEs subsequently by using the same results of the above investigations,noticing that the compositional pattern of PBDEs represents in two dominant congeners,that is,PBDE- 49 and PBDE- 47,which account for 45.39%and 24.68%of ∑_(10) PBDEs,respectively.Both of them belong to the low brominated biphenyls.And,comparatively speaking,the components of the low brominated biphenyls stand far more predominant than those of the high brominated biphenyls.Thus,it can be concluded that the total concentrations of PBDEs in the city's urban areas tend to be higher than those in the suburban areas,and,correspondingly,the urban and the industrial quarters of the city should account for the predominant pollution source of the atmospheric PBDEs.
In order to investigate the actual spatial atmospheric distribution situation in-situ of the pollutants of the polybrominated diphenyl ethers(PBDEs) in Shanghai,we have chosen 15 sampling points in the city in winter.To achieve the goal of our investigation,we have first of all managed to collect the air samples,that is,the PUF(polyurethane foam) passive air samplers for the 3 months in the winter season(from December,2013,to March,2014).And,then,we have managed to make the collected samples treated with Soxhlet extraction and chromatographic purification(pretreated in the lab condition),both in qualitative and quantitative ways,to work out the following 10 targeted components,that is,those of PBDEs(BDE-17,PBEB,BDE-49,BDE-47,BDE-100,BDE-99,BDE-85,BDE-154,BDE- 153 and BDE- 138) respectively in a content concentration range of ∑_(10)PBDEs from 24.18 pg/m~3 to 83.26 pg/m~3,with the mean value of ∑_(10) PBDEs being 61.31 pg/m~3,whereas the average concentrations of ∑_7 PBDEs(BDE- 47,BDE- 99,BDE- 100,BDE-28,BDE- 153,BDE- 154 and BDE- 183) are8.44 pg/m~3(laboratory test of 7 kinds of homologues).The results of the comparative analysis of all the said samples aforementioned show that ∑_(10) PBDEs means in each year are 5.7 pg/m~3,17.28 pg/m~3 and 61.31 pg/m~3 respectively,which represents a clear growing trend during the aforementioned monitoring period.That is to say,the total amount of PBDEs remains in the growing trend for the short term,the long term variation of PBDEs levels will be continued in the near future in the said region.What is more,we have also made a brief analysis of the sources of PBDEs subsequently by using the same results of the above investigations,noticing that the compositional pattern of PBDEs represents in two dominant congeners,that is,PBDE- 49 and PBDE- 47,which account for 45.39%and 24.68%of ∑_(10) PBDEs,respectively.Both of them belong to the low brominated biphenyls.And,comparatively speaking,the components of the low brominated biphenyls stand far more predominant than those of the high brominated biphenyls.Thus,it can be concluded that the total concentrations of PBDEs in the city's urban areas tend to be higher than those in the suburban areas,and,correspondingly,the urban and the industrial quarters of the city should account for the predominant pollution source of the atmospheric PBDEs.
引文
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[14]HAN Wenliang(韩文亮).Polybrominated diphenyl ethers and polychorinated biphenyls in indoor and outdoor air of urban areas(室内与室外空气中的多溴联苯醚和多氯联苯醚)[D].Shanghai:Shanghai University,2009.
[15]SHOEIB M,HARNER T.Characterization and comparison of three passive air samplers for persistent organic pollutants[J].Environmental Science&Technology,2002,36(19):4142-4151.
[16]ZHANG Shangwei(张尚伟),XIA Xinghui(夏星辉),WU Shan(吴山).Toxic effects,sources,distribution and environmental behaviors of 2,2',4,4'-tetrabromodiphenyl ether[J].Journal of Anhui Agricultural Sciences(安徽农业科学),2011,39(5):2882-2887,2981.
[17]CHEN Duohong(陈多宏),BI Xinhui(毕新慧),ZHONG Liuju(钟流举),et al.The seasonal variation character of PBDEs in the atmosphere of the typical e-waste dismantling area[J].Ecology and Environmental Sciences(生态环境学报),2010,19(5):1068-1072.
[18]GEVAO B,GHADBAN AN,UDDIN S,et al.Polybrominated diphenyl ethers(PBDEs)in soils along a rural-urban-rural transect:sources,concentration gradients,and profiles[J].Environmental Pollution,2011,159(12):3666-3672.
[19]ZHU Yunjuan(朱云娟).PBDEs and OCPs ofShanghai City air pollution levels,spatial and temporal distribution and source apportionment(上海市大气中PBDEs和OCPs的污染水平、时空分布以及来源解析)[D].Shanghai:Shanghai Maritime University,2014.
[20]UENO D,KAJIWARA N,TANAKA H,et al.Global pollution monitoring of polybrominated diphenyl ethers shipjack tuna as bioindicator[J].Environmental Science&Technology,2004,38(8):2312-2316.
[2]ZWEIDINGER R A,COOPER S D,ERICKSON M D,et al.Sampling and analysis for semivolatile brominated organics in ambient air[J].Monitoring Toxics Substances ACS Symposium Series,1979,94:217-231.
[3]LUO Xiaojus(罗孝俊),MAI Bixian(麦碧娴),CHEN Shejun(陈社军):Advances on study of polybrominated diphenyl ethers[J].Progress in Chemistry(化学进展),2009,21(2):359-360.
[4]LI Yang(李洋),JI Xiuling(冀秀玲),MA Jing(马静),et al.Preliminary study of PCBs and PBDEs in indoor air samples collected from typical houses in Shanghai[J].Research of Environmental Sciences(环境科学研究),2011,24(5):482-488.[
[5]SONG Xiaoxu(宋晓旭).WANG Zuwei(王祖伟),HU Xiaofang(胡晓芳),et al.Research progress of persistent organic pollutants in different media[J].Northern Environment(北方环境),2012,24(4):135-139.
[6]JIANG Anxi(姜安玺),LIU Liyan(刘丽艳),LI Yifan(李一凡),et al.Air pollution characteristic of polybrominated diphenyl ethers in Heilongjiang Province[J].Journal of Natural Science of Heilongjiang University(黑龙江大学自然科学学报).2004,21(2):97-101.
[7]LIANG Yue(梁越),TANG Xinghua(唐星华),uu Xiaozhen(刘小真),et al.Review on progress of persistent organic pollutants in atmosphere[J].Jiangxi Science(江西科学).2009,27(4):634-638.
[8]MENG Xiangzhou(孟祥周),YANG Chao(杨超),PAN Zhaoyu(潘兆宇),et al.Research advance on polybrominated diphenyl ethers in wastewater and sewage sludge[J].Environmental Science&Technology(环境科学与技术),2011,34(2):102-105.
[9]CHEN Laiguo(陈来国),MAI Bixian(麦碧娴),XU Zhencheng(许振成).et al.Comparison of PCBs and PBDEs concentrations and compositions in the Guangzhou atmosphere in summer[J].Journal of Environmental Sciences(环境科学学报),2008,28(1):150-159.
[10]JIANG Junli(蒋君丽),ZHANG Chengzhong(张承中),MA Wanli(马万里),et al.Pollution characterization and source apportionment of polybrominated diphenyl ethers in autumn air of Xi'an[J].Environmental&ience(环境科学),2011.32(8):2226-2230.
[11]ZHU Xiuhua(朱秀华),WANG Pengyuan(王鹏远),SHI Tai'an(施泰安):Ambient air passive sampling technology for persistent organic pollutants[J].Environmental Chemistry(环境化学),2013,32(10):1956-1966.
[12]JAWARD F M,ZHANG G,NAM J,et al.Passive air sampling of polychlorinated biphenyls,organochlorine compounds and polybrominated diphenyl ethers across Asia[J].Environmental Science and Technology,2005,39(22):8638-8345.
[13]JAWARD F M,FARAR N J,HARNER T,et al.Passive air sampling of PCBs,PBDEs and organochlorine pesticides across Europe[J].Environmental Science and Technology,2004,38(1):34-41.
[14]HAN Wenliang(韩文亮).Polybrominated diphenyl ethers and polychorinated biphenyls in indoor and outdoor air of urban areas(室内与室外空气中的多溴联苯醚和多氯联苯醚)[D].Shanghai:Shanghai University,2009.
[15]SHOEIB M,HARNER T.Characterization and comparison of three passive air samplers for persistent organic pollutants[J].Environmental Science&Technology,2002,36(19):4142-4151.
[16]ZHANG Shangwei(张尚伟),XIA Xinghui(夏星辉),WU Shan(吴山).Toxic effects,sources,distribution and environmental behaviors of 2,2',4,4'-tetrabromodiphenyl ether[J].Journal of Anhui Agricultural Sciences(安徽农业科学),2011,39(5):2882-2887,2981.
[17]CHEN Duohong(陈多宏),BI Xinhui(毕新慧),ZHONG Liuju(钟流举),et al.The seasonal variation character of PBDEs in the atmosphere of the typical e-waste dismantling area[J].Ecology and Environmental Sciences(生态环境学报),2010,19(5):1068-1072.
[18]GEVAO B,GHADBAN AN,UDDIN S,et al.Polybrominated diphenyl ethers(PBDEs)in soils along a rural-urban-rural transect:sources,concentration gradients,and profiles[J].Environmental Pollution,2011,159(12):3666-3672.
[19]ZHU Yunjuan(朱云娟).PBDEs and OCPs ofShanghai City air pollution levels,spatial and temporal distribution and source apportionment(上海市大气中PBDEs和OCPs的污染水平、时空分布以及来源解析)[D].Shanghai:Shanghai Maritime University,2014.
[20]UENO D,KAJIWARA N,TANAKA H,et al.Global pollution monitoring of polybrominated diphenyl ethers shipjack tuna as bioindicator[J].Environmental Science&Technology,2004,38(8):2312-2316.
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